Three dimensional hybrid carbon materials have been prepared using different biomass-derived porous carbons as catalyst supports for growing multi-walled carbon nanotubes (MWCNTs) via a chemical vapor deposition method. The nickel catalyst-loaded supports before and after growing MWCNTs were characterized by scanning and transmission electron microscopy, Fourier transform infrared spectroscopy spectra, and mercury porosimetry. The results show that the grown MWCNTs microstructures are closely related to the porous structures and surface conditions of the carbon supports. By using bamboo as template, a porous carbon support with a large total pore volume, appropriate pore size, and abundant favorable surface functional groups is obtained, which is found to be an ideal support for growing the MWCNTs. Investigation of growth mechanism demonstrated that the combination of appropriate porous structures and surface conditions plays an essential role in catalyst distribution and MWCNTs growth.